Download citation

Share
Download full-text PDF

COMPOSITION AND UTILIZATION OF

MANGO BIO-WASTE
Presentation (PDF Available) · December 2013 with 1,268 Reads
DOI: 10.13140/RG.2.1.3424.4244
Seminar, Department of Food Science and Nutrition, University of Agricultural Sciences,
Dharwad, Karnataka, India, DOI:10.13140/RG.2.1.3424.4244
Cite this publication

Dr. Deepa M Madalageri

o 6.8
o University of Agricultural Sciences, Dharwad

Abstract
Introduction: Mango (Mangifera indica L.) is one of the most cultivated fruit in the
tropical and subtropical region rightly called as king of the fruits. India is the second
largest producer (13.5 MMT) of mango fruits, while the world production was 33.45
MMT (FAO, 2007). Approximately 20% of the mango are processed for products as it is
seasonal, such as puree, nectar, pickles, leather, chutney and canned slices that are
popular world wide. By-products from mango industrial processing represent between
35-60% of the fresh fruit weight (Larrauri et.al., 1996). The by-products are mainly peel,
seed and pulp residues. A regular 3 month production season contributes over 7,500
ton of polluting by-products. The residues represent a waste of nutrients and source of
environmental contaminants. Such by-products could be valuable sources of dietary
fiber (DF), antioxidant compounds and single carbohydrates. Composition of mango
peel: Ajila et al., (2007) showed that mango peel is a rich source of bioactive
compounds such as polyphenols(55-110 mg/g dry peel), carotenoids, vitamin C(188 -
392μg/g dry peel) and E (205-509μg/g dry peel), dietary fibers(45-78%) and enzymes.
Total dietary fiber content was in the range of 40.6–72.5%. Galactose, glucose and
arabinose were the major neutral sugars in insoluble and soluble dietary fibers. Bound
polyphenolic and flavonoid contents were in the range of 8.1–29.5 and 0.101–0.392
mg/g, respectively, and were found to be more in ripe peel than in raw peel. Gallic,
protocatechuic and syringic acids were the bound phenolic acids, and kaempferol and
quercetin were the major flavonoids of the peels. Ferulic acid was identified only in
dietary fiber of Raspuri peels (Ajila and Prasad Rao, 2013). Utilization of mango peel:
Mango peel powder (MPP) could be incorporated up to a 10% level in the formulation of
biscuits without affecting their overall quality. At 10% MPP level incorporation, the
biscuits had TDF of 14.4%, polyphenols of 2630 μg of GAE, carotenoids of 145 μg /g
biscuit powder which are about twofold, fivefold and eightfold more than that of the
control biscuits. The concentration required to obtain 50% DPPH radical scavenging
activity for the biscuits incorporated with 10, 15 and 20% levels of MPP was 10, 4.9 and
4.3 mg, respectively, while it was 250 mg in the case of the control. (Ajila et al., 2008).
The content of phenolics increased from 3.84 to 24.37 mg/g of biscuit incorporated with
deferent levels of MPP. The biscuits incorporated with MPP exhibited an improvement
in their antioxidant properties. Acceptible biscuits with mango flavour were obtained by
incorporating up to 10% MPP ( Ashoush and Gadallah, 2011) Ajila et al., (2010)
revealed that the total dietary fiber, polyphenols, carotenoid content and antioxidant
properties increased in the macaroni prepared with 7.5% incorporation of mango peel
powder. Incorporation of 5% mango peel powder into semolina yielded macaroni with
acceptable quality. Thus, the results suggest that by incorporating mango peel powder,
it is possible to enhance the nutritional quality of macaroni without affecting its cooking,
textural and sensory properties. Composition of mango kernel: Mango kernels make up
about 17-22% of the fruit. The major components of mango kernel are starch, fat and
protein. The oil of mango seed kernel consists of about 44–48% saturated fatty acids
and 52–56% unsaturated. Mango seed kernels have a low content of protein but they
contain the most of the essential amino acids, with highest values of leucine, valine and
lysine. Mango seed is rich in vitamins A, E and C and minerals like Ca, P, Na, K and Mg
.Mango seed kernels were shown to be a good source of polyphenols, phytosterols as
campesterol, sitosterol and tocopherols (Nzikou et al., 2010; Fowomola, 2010;
Kittiphoom, 2012 ) Utilization of mango kernel: Legesse and Emire, (2012) revealed that
maximum reduction of tannins and enhancement of proteins attained by combined
action of soaking and autoclaving process. Flour blends containing up to 30% mango
seed kernel flour were acceptable for biscuit production without adverse effect on
sensory qualities. Ashoush and Gadallah (2011) reveled that mango kernel powder
(MKP) had high content of fat and protein. The biscuits incorporated with MKP exhibited
an improvement in their phenolic and antioxidant properties. Acceptable biscuits with
mango flavor were obtained by incorporating with MKP up to 40%. Arogba (1999)
showed that supplementation of the expensive wheat up to 50 % PMKF ( by weight )
and accompanied with an appropriate recipe for biscuits-making would yield consumer
acceptable products with respect to colour, texture and flavour. Sonwai et al., (2012)
attempted to produce cocoa butter equivalent (CBE) from a blend of mango kernel fat
(MKF) and palm oil mid-fraction (PMF). Similar to cocoa butter, all fat blends contained
palmitic stearic and oleic acids as the main fatty acid components. The triglyceride
compositions of all blends were significantly different from cocoa butter. Conclusion:
Mango peel and kernels, a by-product from mango processing industry, could be
utilized for the preparation of biscuits, macaroni and other food products with improved
functional and nutraceutical properties. Mango peels and seed kernel powders could be
used as a potential source for functional food ingredients. It could be further processed
into therapeutic functional food products. References: Ajila, C.M., Aalami, M.,
Leelavathi, K., and Prasad Rao, U.J.S., 2010, Mango peel powder: A potential source of
antioxidant and dietary fiber in macaroni preparations. Innovative Food Sci. Emerging
Techno. 11: 219-224. Ajila, C.M., Bhat, S.G., and Prasad Rao, U.J.S., 2007, Valuable
components of raw and ripe peels from two Indian mango varieties. Food Chem.
102:1006-1011. Ajila, C.M., Leelavathi, K., and Prasad Rao, U.J.S., 2008, Improvement
of dietary fiber content and antioxidant properties in soft dough biscuits with
incorporation of mango peel powder. J. Cereal Sci., 48: 319-326. Ajila, C.M., and
Prasad Rao, U.J.S., 2013, Mango peel dietary fiber: Composition and associated bound
phenolics. J. Funct. Foods., 5: 444-450. Arogba, S.S., 1999, The performance of
processed mango (Mangifera indica) kernel flour in a model food system. Biores.
Technol., 70: 277-281. Ashoush, I.S., and Gadallah, M.G.E., 2011.Utilization of mango
peels and seed kernels powders as sources of phytochemicals in biscuit. World J. Dairy
Food Sci. 6(1): 35-42. Fowomola, M. A., 2010, Some nutrients and antinutrients
contents of mango (Mangifera indica) seed. African J. Food Sci., 4(8): 472-476.
Hussain, T., Baig, M. Q., and Rashid, H., 1991, Extraction and evaluation of pectin from
mango peel. Pakistan J. Agric. Res., 12(3): 213-216. Kittiphoom, S., 2012, Utilization of
mango seed, mini review. Int. Food Rec. J. 19(4): 1325-1335. Legesse, M. B., and
Emire, S. A., 2012, Functional and physicochemical properties of mango seed kernels
and wheat flour and their blends for biscuit production. African J. Food Sci. Techno., 3
(9): 193-203. Rehman, Z. U., Salariya, A. M., Habib, F., and Shah, W. H., 2004,
Utilization of mango peels as a source of pectin. J.Chem. Soc. Pakistan., 26(1): 73-76.
Sonwai, S., Kaphueakngam, P., and Flood, A., 2012, Blending of mango kernel fat and
palm oil mid fraction to obtain cocoa butter equivalent. J. Food Sci. Technol., 26:197-
212 Srirangarajan, A.N., and Shrikhande, A. J., 1997, Characterization of mango peel
pectin. J. Food Sci., 42: 279-280
 ISHS Acta Horticulturae 992: IX International Mango Symposium

UTILIZATION OF SEED AND PEEL OF MANGO

Authors: S.K. Mitra, P.K. Pathak, H. Lembisana Devi, I. Chakraborty

Keywords: skin, kernel, waste utilization, starch, polyphenols, minerals

DOI: 10.17660/ActaHortic.2013.992.74

Abstract:
Mango consists of between 60-75% flesh; 14-22% seed and 11-18% peel. The relative
proportion of different parts varies with varieties and stage of maturity. Because of 25-40% of
seed and peel in a fruit, a huge amount of waste is generated during industrial processing.
Such by-products are a serious disposal problem, so a commercial utilization for mango peel
and kernels is sought after. Both seed and peel are rich in many useful compounds and could
be utilize in different ways.

Dyeing of cotton and silk yarn with the

extracted dye from the fruit hulls of
mangosteen, Garcinia mangostana Linn
Article (PDF Available) in Fibers and Polymers 8(6):613-619 · December 2007 with 755 Reads
DOI: 10.1007/BF02875998
Cite this publication

Montra Chairat

o 16.67
o Walailak University

John Bremner

o 42.21
o University of Wollongong

Kan Chantrapromma

o 28.83

Abstract
The extracted dye from the dried fruit hulls of mangosteen was used as a natural dye for the dyeing of cotton and silk
yarn. The optimal conditions for dye extraction were to extract the dried fruit hulls of mangosteen at 80°C for 1 hour
with a 15 % w/v citric acid solution in a 1:4 ratio of mangosteen powder to solvent. Cotton dyeing with the extracted
dye from the dried fruit hulls of mangosteen was carried out at 60°C for 60 minutes with a material to liquor ratio of
1:25. The effect on dyeing of mordant type with different mordanting methods was studied. The results showed that
the dyeing of cotton using the post-mordanting method with ferrous sulfate and calcium hydroxide not only provided
better depth of shade but also provided better wash fastness and light fastness than with other mordants (alum; zinc
tetrafluoroborate) or without a mordant. Good fastness properties were also obtained using a post-mordanted silk
with calcium hydroxide.

Discover the world's research

 15+ million members

 118+ million publications
 700k+ research projects

Join for free

Figures - uploaded by Wenlong Zhou
Author content
Content may be subject to copyright.
CIELAB values of dyed cotton fabric subjected to 15 laundering cycles
…

Tensile strength retention (%) of cotton fabric modified with succinic acid/NaH 2 PO 2 (1:1, w/w)
at different concentrations (control, 5, 10, 20, and 30 g l À1 ) and cured at 180 °C for 2 min
[Colour figure can be viewed in the online issue, which is available at wileyonlinelibrary.com.]
…

HPLC anthocyanin profiles (monitored at 520 nm) and UV-vis and MS/MS spectra of major
anthocyanins (peaks 1 and 2) identified in mulberry extracts
…

+4

Selected photo and visible spectra of metal-chelated, diluted mulberry extracts (50-fold volume
of extracts diluted with distilled water). The concentration of metal salts (AlK(SO 4 ) 2 Á12H 2 O,
SnCl 2 Á2H 2 O, FeSO 4 Á7H 2 O, CuSO 4 Á5H 2 O) was 2 g l À1 [Colour figure can be viewed
in the online issue, which is available at wileyonlinelibrary.com.]
…
Content uploaded by Wenlong Zhou
Author content
Content may be subject to copyright.

Download full-text PDF

A method for
dyeing cotton
fabric with
anthocyanin
dyes extracted
from mulberry
(Morus rubra)
fruits
Huayin Wang, Zhirong
Tang and Wenlong Zhou*
Key Laboratory of Advanced
Textile Materials and
Manufacturing Technology
(Ministry of
Education), Zhejiang Sci-Tech
University, Hangzhou, 310018,
China
Email: wzhou@zstu.edu.cn
Received: 31 December 2014;
Accepted: 26 January 2016
For the first time, the natural
anthocyanin dyes (mainly consisting
of cyanidine 3-glycoside) extracted
from
mulberry (Morus rubra) fruits has
been successfully used to dye cotton
fabric, with a dyeing property
performance good enough for
potential commercial applications. In
this study, succinic acid was firstly
incorporated into cotton fabrics by
esterification to the hydroxyl groups
of cellulose, forming an anionic site for
the dyes. The performance of the
modified material was characterised
by Fourier transform infrared
spectroscopy and tensile strength.
Results showed that the tensile
strength of cotton fabrics was mostly
retained after modification. The
anthocyanin extracts from mulberry
fruits were used to study the
dyeability of
the control and modified cotton
fabrics. Red and deep purple
(aubergine) are two main shades of
cotton
fabrics dyed with mulberry fruit
extracts. Most importantly, aubergine
shade is rare in cotton fabrics dyed
with
natural dyes. Modification with
succinic acid clearly increased the
colour strength of the dyed cotton
fabric.
The colour strength of dyed cotton
fabric was improved from 2.7 to 5.3 in
the case of dyeing without
mordants, and from 3.2 to 6.9 in the
case of dyeing with tin mordanting.
Meanwhile, the colour fastness was
improved by 0.5–2 grades with
increasing succinic acid concentration
in the finish solution. The colour
fastness to perspiration, crocking,
light, and washing of fabric dyed with
simultaneous tin mordanting and
modified with 30 g l
1

of succinic acid was found to be

acceptable, with a grey scale grade of
at least 3. As
for home laundering, neutral soapy
solution was more acceptable than
alkaline soapy solution.

Coloration
Technology
Society of Dyers and Colourists

Introduction
Natural dyes/pigments are
biodegradable and curative, are
extracted under mild reaction
conditions, and present no
disposal problems owing to their
high environmental
friendliness [1–3]. The dyeing of
cotton fabric with natural
dyes with a colour performance
good enough for commer-
cial uses has attracted much
research.
Cotton is considered to be one of
the most important
natural polymers and is widely
used in various production
processes, especially in the textile
industry. At a molecular
structure level, cotton is a
carbohydrate homopolymer
consisting of b-D-glucopyranose
units joined together by
b-1,4-glycosidic linkages [4,5].
The hydrogen bond network
formed between the polymer
components involves a large
number of hydroxyl groups and
ether oxygen [6]. Cotton
does not contain sufficient and
appropriate ionic sites to fix
cationic or anionic dyes through
Coulomb forces. Recent
developments in natural dyeing
mainly rely on the modi-
fication of cotton fabrics using
various pre- and post-
treatment agents to improve
colour yield, fastness, and
functional characteristics. A
number of investigations have
indicated that pretreatment of
cotton fabrics with cationic
agents, e.g. poly(ethyleneimine)
[7], triethylamine [8],
polyaminochlorohydrin
quaternary ammonium [9], and 3-
chloro-2-hydroxypropyltrimethyl
ammonium chloride [10],
enhances the colour strength and
fastness properties of
dyeing over untreated cotton
fabrics to a significant extent
for many natural dyes. Moreover,
natural polymers, such as
chitosan [11,12] and bovine
serum albumin [7] have been
investigated as pretreatment
agents for the modification of
cotton fabrics. Moreover,
mordanting [13–15], enzyme-
assisted dyeing [16,17], and
sonicator-assisted dyeing [18]
have also been considered as
useful approaches for creating
affinity between natural dyes and
cotton fibres [19].
Mulberry (Morus rubra) is a plant
native to Asia and
widely cultivated in Southern
Europe for centuries because
of its wide usage for many
purposes. In traditional Chinese
medicine, dried mulberry fruits
have been used for their
tonic and sedative effects, like the
leaves and root bark of
mulberry [20]. The mulberry fruits
contain various polyphe-
nols with physiological functions
that offer protection to
humans [21,22]. Anthocyanins
and flavonols are two major
polyphenolic compounds in
mulberry fruits. The main
flavonols in mulberry fruits
include quercetin, morin, and
myricetin [23,24]. The main
anthocyanins include cyanidin
3-glycoside and pelargonidin 3-
glycoside, which are respon-
sible for the colouring of fruits and
fruit products [25].
Research has shown that
anthocyanins have strong oxida-
tion resistance [26] and
antimicrobial properties [27] and
provide UV protection [28,29].
Anthocyanins can also
inhibit the growth of cancerous
cells and inflammation,
and have anti-obesity effects
[30,31]. In spite of the great
application potential of mulberry
fruits in the food, phar-
maceutical, and cosmetic
industries, their direct application
in textiles is limited as the
extracted pigments lack affinity
to the natural polymer, especially
to cotton fibres. The dyed
cotton fabric is unable to gain
satisfactory colour strength
(K/S) and sustain home
laundering. Therefore, further
investigation is required.
In the present study, anthocyanin
dyes were successfully
applied to cotton fabrics, and
deep purple (aubergine) and
red shades were obtained. Of
these, deep purple (aubergine)
is especially rare in cotton fabrics
dyed with natural dyes.
An anionic agent (succinic acid
was used in this paper)
containing carboxyl groups was
introduced into the cotton
222 © 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol., 132,
222–231
doi: 10.1111/cote.12212
fabrics to increase the affinity of
the dyes to the fabric, thus
enhancing the K/S values of dyed
cotton fabrics. Dye
structures, colorimetric data, and
the colour fastness of
the dyed cotton fabrics are
examined, and the correspond-
ing properties are discussed.
Experimental
Materials and reagents
The bleached fabric used in this
work was a plain woven
100% cotton (42 yarns cm
1

in the warp direction and

19 yarns cm
1

in the weft direction, 190 g m

2

), which was
obtained from local markets in
Hangzhou, China.
Methanol, succinic acid, sodium
hypophosphite, sodium
acetate, acetic acid, potassium
chloride, hydrochloric acid,
trifluoroacetic acid (TFA),
potassium-aluminium sulfate
(alum), ferrous sulfate, stannous
chloride, and copper
sulfate were obtained from Aladin
(China). All the above
chemicals were analytical grade.
Acetonitrile (HPLC gradi-
ent grade) and formic acid (HPLC
gradient grade) were
obtained from Merck (Germany).
High-purity water was
obtained by passing water though
a Milli-Q treatment
system (Millipore, USA), and the
HPLC mobile phase was
prepared using Milli-Q water.
Extraction of mulberry dyes
The fresh mulberry fruits were
crushed with a mortar and
mixed with solvent
(methanol/TFA/H
2

O 80:0.5:19.5 v/v/v),
keeping a material-to-liquor ratio
of 1:2. Extraction was
carried out at a temperature of 50
°C for 2 h, followed by
filtration. The filtrate was diluted
with distilled water (1:4 v/
v) and later used for dyeing.
The concentration of mulberry
dye solution was calcu-
lated from the total anthocyanin
content (TAC) using the
pH differential method and
expressed as cyanidin 3-gluco-
side (Cy 3-glc) equivalents
according to the equation [32,33]
1
Anthocyaninconcentrationðmgl
AM DF 1000
Þ¼ w
 ð1Þ
em 1
where A is the absorbance value
in the visible region, equal
to ðAkmax  A700ÞpH1:0 ðAkmax  A700
ÞpH4:5 , which corresponds
to sodium acetate–acetic acid
buffer solution with pH 4.5
and potassium chloride–
hydrochloric acid buffer solution
with pH 1.0 to dilute the
anthocyanin extracts, M
w

is the
molecular weight (g mol
1

) of Cy 3-glc (449.2 g mol

1
in
the analysis), DF is the dilution
factor, e
m

is the molar
extinction coefficient (26 900 for
Cy 3-glc), and d is the path
length of the cuvette (1 cm in the
analysis). Triplicate
assays were applied.
The total anthocyanin content
(TAC) in the dyeing
solution was 384.1  35.4 mg l
1

.
High-performance liquid
chromatography/tandem mass
spectrometry
The anthocyanins were identified
in mulberry fruit extracts
by liquid chromatography with
photodiode array detection/
electrospray ionisation tandem
mass spectrometry (HPLC-
DAD-ESI-MS/MS). HPLC/DAD
experiments were performed
on a 1260 Infinity HPLC
instrument (Agilent Technologies,
USA). For analysis, separation of
anthocyanins were
carried out on an Agilent Zorbax
SB-C
18

column
(4.6 9 250 mm, 5 lm) (Agilent
Technologies) equipped
with a C
18

guard column (Agilent

Technologies,). The
column oven temperature was set
at 35 °C. The mobile
phase consisted of 10% formic
acid (solvent A) and 100%
CH
3

CN (solvent B). For separation of

anthocyanin extracts,
the elution conditions were set as
follows: isocratic elution
0% B, 0–10 min; linear gradient
from 0% B to 10% B, 10–
20 min; 12% B, 20–40 min; 100%
B, 40–50 min, 100% B,
60 min; flow rate 1.0 ml min
1

; injection volumes 10 ll.

The detected wavelength was 520
nm. MS and MS/MS
experiments were performed
using an LCQ Fleet mass
spectrometer (Thermo Fisher
Scientific, USA) and electro-
spray ionisation (ESI). The MS
analytical parameters were
as follows: polarity positive; ion
source turbo spray (ESI);
capillary temperature 350 °C;
capillary voltage 60 V; spray
voltage 4.5 vV; full-scan range
from m/z 400 to 1200. An
MS
2

scan of the most abundant ion

uses a relative collision
energy of 20%.
Modification of cotton fabrics
The cotton fabric was first
impregnated in a finish solution
containing succinic acid and
sodium hypophosphite of
specified concentration with
succinic acid:sodium
hypophosphite = 1:1 (w/w). The
fabric was then passed
through two dips and two nips in
a laboratory padder. The
impregnated fabric was dried at
90 °C for 3 min and finally
cured at 180 °C for 2 min in a
curing oven [34]. The wet
pick-up of the cotton fabric was
approximately 80%.
Dyeing
The dyeing experiments were
carried out in a dyeing
solution with the liquor to fabric
ratio of 50:1, at 60 °C for
60 min. Both the direct and
simultaneous mordanting
dyeing modes were performed.
The calculated amount of
mordant (10% of the weight of
fabric, owf) was added to the
dyebath. No adjustment of pH
value was made. The dyed
fabric was rinsed with cold water
and finally dried at 50 °C.
Fourier transform infrared
spectral analysis
The structural changes occurring
in the cotton fabrics were
monitored by Fourier transform
infrared (FTIR) spec-
troscopy. A PerkinElmer System
2000 FTIR spectropho-
tometer (PerkinElmer, USA) was
used to collect the
transmission spectra of all powder
samples in the wave
number range 400–4000 cm
1

. The FTIR spectra of the

powders were collected using the
KBr pellet technique. The
resolution for all the infrared
spectra was 4 cm
1

, and there
were 100 scans for each
spectrum.
Tensile strength
The tensile strength of cotton
fabric was measured accord-
ing to the ASTM D5035-11(2015)
[35], and was tested in the
warp direction only. Five
specimens were used for each
data point.
Colour evaluation
Colour values of fabrics were
evaluated by mean of colour
strength (K/S) and CIELAB
parameters (L*, a*, b*, C*, and
h). CIELAB values were
determined by illuminant D65 on
a
Datacolor SF600
spectrophotometer (Datacolor
Interna-
tional, USA), with a sample
diameter of 10 mm (geome-
try d/10°). The colour strength
(K/S) was calculated on the
basis of the Kubelka–Munk
equation
Wang et al. Anthocyanin dyeing of cotton
fabric
© 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol.,
132, 2 2 2 –231 223
ð1  RÞ2
K=S ¼
ð2Þ
2R
where K is the adsorption
coefficient, R is the reflectance of
the dyed sample, and S is the
scattering coefficient.
In uniform CIELAB space,
L* corresponds to brightness
(100 = white, 0 = black), a* to
the red-green coordinate
(positive sign = red, negative sign
= green), and b* to the
yellow-blue coordinate (positive
sign = yellow, negative
sign = blue); C* is the
quantitative parameter of the
chroma
of the colour, and h is the
quantitative parameter of the hue
of the colour.
The colour fastness of dyed
cotton fabrics was tested
according to AATCC standard
methods. Light fastness tests
were carried out according to
AATCC 16-2004 [36]. The
colour change of the samples was
assessed against the grey
scale and blue wool standard.
Colour fastness to washing,
crocking fastness, and
perspiration fastness tests were
carried out according to AATCC
61-2009 [37], AATCC 8-
2007 [38], and AATCC 15-2009
[39] respectively. The
colours of the specimens were
rated by referencing to the
grey scale for colour change. The
staining on each original
fabric was rated by means of the
grey scale for staining.
Colour durability
The durability of the dyed cotton
fabric against repeated
launderings was evaluated by
washing cotton fabrics
according to AATCC 61(2A)-2009
[40], with minor modifi-
cation. Washing was carried out
using an aqueous solution
of 5 g l
1

of neutral detergent (Omo brand;

Unilever, China)
or alkaline detergent (Diao brand;
Nice Group, China) at
49 °C for a duration of 45 min
using a material:liquor ratio
of 1:50. The pH values of the
neutral and alkaline soapy
solutiona were 7.5 and 10.2
respectively. After each
washing cycle, the fabric was
dried at 70 °C for 15 min
and the colour values were
evaluated. The dyed cotton
fabrics were subjected to one,
five, ten, and 15 consecutive
washing/drying cycles.
Results and discussion
Mechanism
Polycarboxylic acids are the most
promising non-formal-
dehyde durable press finishes for
cotton fabrics [41,42]. In
some preliminary dyeing
experiments, we grafted or
crosslinked citric acid, tartaric
acid, 1,2,3,4-butanetetracar-
boxylic acid (BTCA), or succinic
acid onto cotton fabrics,
and found that the dyeability of
natural anthocyanin dyes
for the modified cotton fabrics
was improved significantly.
However, more than 35% loss of
tensile strength of cotton
fabrics was evident after
modification with BTCA, citric
acid, or tartaric acid with an acid
concentation of 30 g l
1

,
while the loss of tensile strength
of cotton fabrics modified
with succinic acid was about 20%,
mostly owing to no
substantial crosslink formed
between cellulose molecules.
Therefore, succinic acid was
considered to be an adoptable
agent for modification of cotton
fabrics and was investi-
gated in this paper. Succinic acid
is a dicarboxylic acid
that is capable of forming ester
linkages with hydroxyl
groups of cellulose molecules
[34,43]. The modification
mechanism of cotton fabrics using
succinic acid in the
presence of sodium
hypophosphite (catalyst) is shown
in
Figure 1.
During the dye adsorption
process, different kinds of
interaction between substrate and
dye, such as chemical
bonding, ion exchange, hydrogen
bonds, hydrophobic
attractions, Van der Waals forces,
physical adsorption,
aggregation mechanisms, dye–
dye interactions, etc., may
occur simultaneously [44]. For
unmodified cotton fabrics,
hydrogen bonds between –OH of
cotton and –OH of
anthocyanin dyes and Van der
Waals forces were the main
factors during anthocyanin dye
adsorption. In acidic solu-
tion (pH < 3.0), the flavylium
cation is the predominant
structural form of anthocyanins
[45–47]. Thus, the adsorp-
tion was driven by strong ionic
interaction (Coulomb force)
between the negatively charged –
COO


groups anchored at
the modified cotton fabrics and
cationic anthocyanin dyes
in solution (Figure 2).
Fourier transform infrared
analysis
The FTIR spectra of cotton with
and without modification
with succinic acid are shown in
Figure 3. A strong O–H
stretching absorption at 3396 cm
1

with a broad peak

appeared in spectrum of cotton.
The bands at 2904 cm
1

were assigned to C–H bond

stretching absorption of cellu-
lose. The C–O–C stretching
absorption was around
1064 cm
1

. The characteristics of FTIR

absorption are
consistent with those of typical
cotton cellulose [12]. After
modification with succinic acid,
absorption around
1730 cm
1

appears in the spectrum of

cotton, which is
CH2 COOH Cell OH
Catalyst, heat
COOH
CH2
CH2 COOCell
COOH
CH2
Figure 1 Reaction of the modification
of cotton fabrics
CH2
CH2
COOCell
COO– + OH
Modified cotton Anthocyanin dye
Figure 2 Proposed mechanism for the
main adsorption of antho-
cyanin dyes on modified cotton
4000
a
b
c
d
e
Transmittance, %
3500
3396
2904
1730
1064
3000 2500 2000
Wave number, cm–1
1500 1000 500
Figure 3 FTIR spectra of cotton fabric
treated with succinic acid/
NaH
2

PO
2

(1:1, w/w) at SA concentrations of (a)

control, (b) 5 g l
1

,
(c) 10 g l
1

, (d) 20 g l
1

, and (e) 30 g l
1

and cured at 180 °C for

2 min [Colour figure can be viewed in
the online issue, which is
available at wileyonlinelibrary.com.]
Wang et al. Anthocyanin dyeing of cotton
fabric
224 © 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol., 132,
222–231
attributed to the introduction of
C=O groups of carboxylic
acid by the modification [48]. The
intensity of absorption at
1730 cm
1

increased with increase in the

succinic acid
concentration in the finish
solution, indicating successful
esterification of the succinic acid
to cotton cellulose.
Tensile strength
The effect of succinic acid
treatment on the tensile strength
of the cotton fabrics is shown in
Figure 4. After finishing, it
is noted that the tensile strength
of the cotton fabric slightly
decreases with increasing
concentration of succinic acid in
the finish solution. A 21.5  7.1%
loss of tensile strength is
observed at a concentration of 30
gl
1

of succinic acid in
the finish solution. Such tensile
strength loss of the cotton
fabric is considered to be low for
application of the dyed
cotton fabric in the area of
apparel, where improved colour
strength (K/S) or wrinkle
resistance property is of impor-
tance at the cost of even up to
30% of the original strength of
the cotton fabrics [49]. Therefore,
considering the tensile
strength and K/S data in Figures 4
and 8, it appears that
30 g l
1

of succinic acid in the finish

solution produced the
optimum, or most improvement
in, colour strength (K/S) o f
the cotton fabrics dyed with
mulberry extracts in this paper.
Main anthocyanins of fruit
extracts
Anthocyanins in mulberry extracts
were identified by
HPLC-DAD-ESI-MS. Figure 5 shows
the HPLC profile of
the anthocyanins present in an
extract of mulberry fruits.
The specific data obtained by
HPLC-DAD-ESI-MS analysis
are summarised in Table 1. As
shown in Figure 5, at least
four anthocyanins exist in the
extracts. Their retention
times are 24.0, 24.7, 26.3, and
27.7 min respectively. Two
major anthocyanins, peaks 1 and
2, took up 61.5 and 37.1%
of the total anthocyanin content,
respectively, in the
chromatogram [50]. For the
anthocyanins, UV-vis spectra
and HPLC retention time can be
used to determine the
chemical structure [51].
Compounds associated with
peaks
1 and 2, showing k
max

at 279, 331, 516 nm and 280,

330,
517 nm respectively, were related
to cyanidin-derived
anthocyanins. Similarly, peaks 3
and 4 (k
max
at 275, 329,
100
90
80
70
60
50
Control 5 10 20 30
Succinic acid concentration, g l–1
Tensile strength retention, %
Figure 4 Tensile strength retention (%)
of cotton fabric modified
with succinic acid/NaH
2

PO
2

(1:1, w/w) at different concentrations

(control, 5, 10, 20, and 30 g l
1
) and cured at 180 °C for 2 min
[Colour figure can be viewed in the
online issue, which is available
at wileyonlinelibrary.com.]
500
500
400
300
200
100
0
250
100
287.1
449.2
287.2
449.2
595.2

HO HO
OH
OH
OH
OH
OH
OH
OH
OH
O
⊕
⊕
O O
O
O
HO
HO
HO
O
O
O
OH
OH
OH
OH
OH
OH
80
Relative abundance
60
40
20
0
100
80
Relative abundance
60
40
20
0
200 400 600 800
m/z
m/z = 287
m/z = 287
m/z = 162
m/z = 146
m/z = 162
1000 1200 1400 200 400 600 800
m/z
1000 1200 1400
300 350 400 450
Wavelength/nm
Absorbance
Absorbance
500 550 600 250 300 350 400 450
Wavelength/nm
500 550 600
400
300
100
0
0 1 0
2 0 3
0
3 4
1 250
200
150
100
50
0
2
Minute
40 50 60
200
mau
Figure 5 HPLC anthocyanin profiles
(monitored at 520 nm) and UV-vis and
MS/MS spectra of major anthocyanins
(peaks 1 and 2) identified
in mulberry extracts
Wang et al. Anthocyanin dyeing of cotton
fabric
© 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol.,
132, 2 2 2 –231 225
501 nm for peak 3, k
max
at 275, 329, 503 nm for peak 4)
were assigned as pelargonidin-
derived anthocyanins. Peak 1
showed a molecular ion at
m/z 449 that produced a unique
MS
2

fragment at 287 (cyanidin)

(Figure 5). The direct loss of
162 amu indicated the separation
of a sugar residue.
Supported by the existence of a
shoulder at around
440 nm in the UV-vis spectrum of
peak 1 (Figure 5), peak
1 is characteristic of 3-
glycosylate, suggesting its
identity to
cyanindin 3-glucoside (Figure 5).
Similar observations to
those described for peak 1 were
made regarding fragmen-
tation pattern, absorption
spectrum, and sugar identifica-
tion, and peaks 2, 3, and 4 were
identified as cyanidine 3-
rutinoside (Figure 5), pelargonidin
3-glucoside, and
pelargonidin 3-rutinoside
respectively. The specific data
of the four anthocyanins identified
(Table 1) were in
accordance with previous results
[21, 52, 53].
Very few other pigment
compounds (monitored at
520 nm) were found. Among the
anthocyanins in mulberry
extracts, cyanidine 3-glycoside
(cyanidine 3-glucoside and
cyanidine 3-rutinoside) was the
major anthocyanin struc-
ture and took up 98.6% of the
total anthocyanin content in
the chromatogram. Even without
further purification, the
mulberry extracts can still be
considered as a single-
component anthocyanin dye for
cotton dyeing in this
study.
The main characteristic of
anthocyanins and anthocyani-
dins with o-di-hydroxyl groups in
the B ring (Cy, Dp, Pt) is
their ability to form metal-
anthocyanin complexes [54].
Metals have already been used to
stabilise the colour of
cyanidin, delphinidin, and
petunidin, which have more
than one free hydroxyl group in
the chromane ring and are
capable of metal chelation [55].
The most common metals
in anthocyanin complexes are tin,
copper, ferrous, alu-
minium, and other metals [56,57].
In this paper, tin-,
copper-, ferrous-, and aluminium-
ion-chelated, diluted
mulberry extracts are shown in
Figure 6. As shown in
Figure 6, with the addition of
metal salts (except ferrous
salts), the bathochromic
maximum absorption wavelength
of the diluted mulberry extracts
shifts 4–37 nm and the
absorbance increases
significantly. The hyperchromic
effect
of the anthocyanin solution by
metal is evident. Here, the
hyperchromic effect of tin–
anthocyanin complexes is most
significant. The absorbance value
of diluted mulberry
extracts is increased from 0.6 to
2.3 at k
max

in the visible
range. The colour of the diluted
mulberry extracts also
changes from red to purplish red
after tin–anthocyanin
complex formation. The colour of
ferrous–anthocyanin
complexes is yellowish green
owing to the effect of the
natural yellow colour of ferrous
ion, while alum and copper
salts rarely change the colour of
the extract. As the purple
shade is rare in cotton fabrics
dyed with natural dyes, we
will choose only tin salt and focus
our discussion on tin salt
as a mordant in this paper. By
increasing the amount of tin
salt from 0.5 to 15% (owf) in the
dyebath, the shade of the
dyed fabric shifted from red to
deep purple at 10% (owf),
after which no obvious shade
change was observed in our
Table 1 Retention times and
percentage peak areas of chemicals in
HPLC anthocyanin profiles (monitored
at 520 nm), maximum absorption
(k
max

) of chemicals in UV-vis spectra,

m/z values of molecular ions and
fragmentation patterns in MS/MS
spectra, and deduced chemicals in
mulberry extracts
Peak Retention time, min Peak area,
% (520 nm) k
max

,nm [M
+

] ( m/z) M S
2

of [M
+

] ( m/z) Compound
1 24.0 61.5 516, 279, 331 449 287
Cyanidine 3-glucoside
2 24.7 37.1 517, 280, 330 595 449,
287 Cyanidine 3-rutinoside
3 26.3 1.0 501, 275, 329 433 271
Pelargonidin 3-glucoside
4 27.7 0.4 503, 275, 329 579 433, 271
Pelargonidin 3-rutinoside
Control Copper Ferrous
Tin Aluminium
0.0
400 450 500 550
Wavelength, nm
600 650 700 750 800
0.5
1.0
1.5
Absorbance
2.0
2.5
551 Control
Tin
Copper
526
516
514
Aluminium
Ferrous
Figure 6 Selected photo and visible
spectra of metal-chelated, diluted
mulberry extracts (50-fold volume of
extracts diluted with distilled
water). The concentration of metal
salts (AlK(SO
4

)
2

12H
2

O, SnCl
2

2H
2

O, FeSO
4

7H
2

O, CuSO
4

5H
2

O) was 2 g l
1

[Colour figure can be

viewed in the online issue, which is
available at wileyonlinelibrary.com.]
Wang et al. Anthocyanin dyeing of cotton
fabric
226 © 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol., 132,
222–231
preliminary tests. Thus, 10% (owf)
tin salt was used in the
mordanting dyebath in our
subsequent experiments.
In the mordanting dyeing process,
metallic salts (stannous
chloride was used in this paper)
are used not only to stabilise
anthocyanins but also to fix
natural dyes to cotton cellulose as
a mordant. Thereby, they improve
the dye uptake of the fabric
and help improve the colour
fastness [58,59].
Dyeing
Effect of dyeing time on colour
strength
The colour strength (K/S) of
modified cotton fabrics dyed
with mulberry extracts is related
to the dyeing time to a
great extent. Figure 7 shows a
plot of K/S against dyeing
time by the direct and
simultaneous mordanting dyeing
method. It can be seen that the
rate of K/S was quite fast in
the first 5 min of dyeing, and then
tended to be constant for
the direct dyeing method. As for
simultaneous mordanting
dyeing (tin used in this paper),
the rate of K/S was also quite
fast in the initial stage of dyeing,
and tended to be constant
after 40 min. The plots indicate
that 5 min dyeing time and
40 min dyeing time are
reasonable for direct and simulta-
neous mordanting dyeing of
cotton fabrics with mulberry
extracts respectively.
Effect of succinic acid
modification on colour strength
The relationship between the
succinic acid concentration in
the modifying solution and the
dyed colour strength (K/S) i s
illustrated in Figure 8. It can be
seen from Figure 8 that
unmordanted (mordant-free) dyed
cotton fabric showed a
lower dye uptake (according to
the K/S) compared with the
simultaneous mordanting dyed
cotton fabric with the same
natural anthocyanin dyes.
Furthermore, the results demon-
strate that the K/S value is
significantly affected by the
succinic acid concentration in the
finish solution used for
cotton fabric modification. The
K/S value of dyed cotton fabric
was improved from 2.7 to 5.3 for
dyeing without mordants,
and from 3.2 to 6.9 for
simultaneous mordanting dyeing.
It
can also be seen from Figure 8
that the K/S value increased
sharply as the succinic acid
concentration in the finish
solution increased to 20 g l
1

for dyeing without mordants or

to 10 g l
1

for simultaneous mordanting

dyeing. The higher
succinic acid concentration may
lead to a higher K/S value,
but the tensile strength of the
cotton fabrics would decrease
simultaneously. A concentration
of 30 g l
1

of succinic acid
in the finish solution was
acceptable, with 21.5  7.1%
tensile strength loss of the cotton
fabric. The corresponding
colorimetric parameters of the
dyed cotton fabrics in Table 2
show that the increased K/S was
reflected in lower L* values,
but the a*, b*, C*, and h* values
showed no distinct changes,
which means the modification of
cotton fabric with succinic
acid would not cause any obvious
change in shade after
dyeing with mulberry extracts.
The relevant fastness of the
dyed cotton fabrics is also given
in Table 2.
As shown in Table 2, colour
fastness to light, perspira-
tion, and crocking was mostly in
the range 3–4.5 (fair to
very good), except for the direct
dyeing of the control and
the cotton fabric modified with 5
gl
1

of succinic acid, the

grades of which were 2 (poor) and
2.5 (poor) respectively,
which means that the colour
fastness to light, perspiration,
and crocking of most cotton
fabrics dyed with natural
anthocyanin dye was acceptable
after modification of the
cotton fabric with more than 10 g
l
1

of succinic acid in
the finish solution. However, the
wash fastness of most of
8
(a)
(b)
Control
5 g l–1
10 g l–1
20 g l–1
30 g l–1
Control
5 g l–1
10 g l–1
20 g l–1
30 g l–1
7
6
5
K/S value, 530 nm
4
3
2
1
0 1 0 2 0 3
0
Dyeing time, min
40 50 60
8
7
6
5
K/S value, 550 nm
4
3
2
1
0 10 20 30
Dyeing time, min
40 50 60
Figure 7 Effect of dyeing time on
colour strength (K/S) of the
control and modified cotton fabrics:
(a) mordant-free dyeing; (b)
mordant tin dyeing. Modification
conditions: succinic acid/
NaH
2

PO
2
(1:1, w/w) at different concentrations
(control, 5, 10, 20,
and 30 g l
1

) and cured at 180 °C for 2 min.

Dyeing conditions: dye
concentration 1.9  0.2% owf (TAC),
material-to-liquor ratio 1:50,
temperature 60 °C, amount of
mordant tin salt 10% owf [Colour
figure can be viewed in the online
issue, which is available at
wileyonlinelibrary.com.]
Mordant free
7.0
3.2
4.2
5.5
6.3
6.9
5.3
5.0
3.2
3.0
2.7
Mordant tin
6.0
5.0
K/S value
4.0
3.0
0.0 5.0 10.0 15.0
Succinic acid,
g
l–1
20.0 25.0 30.0
Figure 8 Effect of succinic acid in
finish solution on the colour
strength (K/S) of dyed cotton.
Modification conditions: succinic
acid/NaH
2

PO
2

(1:1, w/w) at different concentrations

(0, 5, 10, 20,
and 30 g l
1

) and cured at 180 °C for 2 min.

Dyeing conditions: dye
concentration 1.9  0.2% owf (TAC),
dyeing time 60 min, material-
to-liquor ratio 1:50, temperature 60
°C, amount of mordant tin salt
10% owf. Dyeing method: direct
dyeing and simultaneous mor-
danting dyeing [Colour figure can be
viewed in the online issue,
which is available at
wileyonlinelibrary.com.]
Wang et al. Anthocyanin dyeing of cotton
fabric
© 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol.,
132, 2 2 2 –231 227
the dyed cotton fabrics ranged
from only 1 to 2 (very poor to
poor), which is unsatisfactory, the
exception being cotton
fabric modified with 30 g l
1

of succinic acid in the finish

solution and mordanted with
tannous chloride, the grade of
which was 3 (fair). It is also quite
apparent from the data in
Table 2 that the fastness is
improved 0.5–2 grades with
increase in the succinic acid
concentration in the finish
solution.
Table 2 Colorimetric parameters and
fastness of dyed cotton fabrics
Succinic acid, g l
1

Mordant
L* a* b* C* h*
WF
a

Perspiration Crock
LF
d

CC
b

CS
c

CC
b

CS
c

Dry Wet
0 Free 54.6 32.4 6.6 33.1 348.6 1 3
3 2 4.5 3 3
5 Free 52.8 32.1 5.9 32.7 349.6 1.5
3.5 3 2.5 4.5 3 4
10 Free 52.7 33.4 5.6 33.9 350.5
1.5 3.5 3 3 4.5 3.5 4
20 Free 48.7 39.2 3.9 39.4 354.3
1.5 3.5 3.5 3 4.5 3.5 4
30 Free 46.9 36.9 3.0 37.0 355.3 2
3.5 3 3 4.5 3.5 4
0 Tin 49.2 22.4 23.6 32.6 313.5 1.5
3 3.5 3.5 4.5 3 3.5
5 Tin 43.5 14.6 17.1 22.4 310.5 1.5
3.5 4 3.5 4.5 3.5 3.5
10 Tin 39.6 15.4 17.2 23.1 311.8 2
4 4 4 4.5 3.5 3.5
20 Tin 39.1 21.8 22.3 31.2 314.4
2.5 4 4 4 4.5 3.5 4
30 Tin 37.1 16.4 21.8 27.3 306.9 3
4 4.5 4 4.5 3.5 4.5
a Wash fastness.
b Colour change.
c Colour staining.
d Light fastness.
7.2
(a) (b)
(c) (d)
5.3
Control
5gl
–1
30 g l
–1
Control
5gl
–1
30 g l
–1
3.0
2.7
0.4 0.3 0.2
0.2
6.4
5.6
4.8
4.0
3.2
K/S value
2.4
1.6
0.8
0.0
–2.0 0.0 2.0 6.0 8.0
Washing cycles
10.0 12.0 14.0 16.04.0
7.2
5.3
3.0
2.7
0.5 0.3 0.3 0.3
6.4
5.6
4.8
4.0
3.2
K/S value
2.4
1.6
0.8
0.0
–2.0 0.0 2.0 6.0 8.0
Washin
g
cycles
10.0 12.0 14.0 16.04.0
7.2
6.9
6.9
4.2
3.2
2.5
0.7
0.5
0.4 0.3
0.3
4.7
4.2
4.2
3.3 3.3
1.8
2.2
2.5
3.1
3.2
2.1 1.5 1.3
1.2
Control
5gl
–1
30 g l
–1
Control
5gl
–1
30 g l
–1
6.4
5.6
4.8
4.0
3.2
K/S value
2.4
1.6
0.8
0.0
–2.0 0.0 2.0 6.0 8.0
Washing cycles
10.0 12.0 14.0 16.04.0
7.2
6.4
5.6
4.8
4.0
3.2
K/S value
2.4
1.6
0.8
0.0
–2.0 0.0 2.0 6.0 8.0
Washin
g
cycles
10.0 12.0 14.0 16.04.0
Figure 9 Influence of laundering cycles
on the colour strength (K/S) of control
and modified (5 and 30 g l
1

) cotton fabrics: (a) mordant free,

washed in neutral soapy solution; (b)
mordant tin, washed in neutral soapy
solution; (c) mordant free, washed in
alkaline soapy solution; (d)
mordant tin, washed in alkaline soapy
solution. Modification conditions:
succinic acid/NaH
2

PO
2

(1:1, w/w) at different concentrations

(control, 5, and 30 g l
1

) and cured at 180 °C for 2 min.

Dyeing conditions: dye concentration
1.9  0.2% owf (TAC), dyeing time 60
min,
material-to-liquor ratio 1:50,
temperature 60 °C, amount of
mordant tin salt 10% owf. Dyeing
method: direct dyeing and
simultaneous
mordanting dyeing [Colour figure can
be viewed in the online issue, which is
available at wileyonlinelibrary.com.]
Wang et al. Anthocyanin dyeing of cotton
fabric
228 © 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol., 132,
222–231
Table 3 CIELAB values of dyed cotton
fabric subjected to 15 laundering
cycles
Cotton fabric Mordant Soapy solution
L* a* b*
C* h*
Undyed 92.1 0.4 0.7 0.9 238.8
Control Free Original 54.6 32.4 6.6
33.1 348.6
Neutral 79.2 4.3 14.4 15.0 286.8
Alkaline 82.7 3.1 16.4 16.7 280.8
Control Tin Original 49.2 22.4 23.6
32.6 313.5
Neutral 60.6 9.3 18.9 21.1 296.1
Alkaline 80.3 5.7 16.8 17.8 288.9
Modified
a

Free Original 54.2 24.8 7.2 25.8

343.7
Neutral 77.4 3.3 11.3 11.8 286.2
Alkaline 79.8 0.5 10.0 10.0 273.0
Modified
a

Tin Original 37.1 16.4 21.8 27.3

306.9
Neutral 47.4 12.6 21.4 24.9 300.5
Alkaline 76.3 4.6 10.5 11.4 293.6
a Cotton fabrics were modified with 30 g l
1

of succinic acid.
0 cycle
(a)
(b)
(c)
(d)
1 cycle 5 cycles 10 cycles 15 cycles
0 cycle 1 cycle 5 cycles 10 cycles 15
cycles
0 cycle 1 cycle 5 cycles 10 cycles 15
cycles
0 cycle 1 cycle 5 cycles 10 cycles 15
cycles
Figure 10 Selected dyed cotton fabrics
modified with 30 g l
1

of succinic acid subjected to specified

laundering cycles: (a) mordant free,
washed in neutral soapy solution; (b)
mordant tin, washed in neutral soapy
solution; (c) mordant free, washed in
alkaline soapy solution; (d)
mordant tin, washed in alkaline soapy
solution [Colour figure can be viewed
in the online issue, which is available
at
wileyonlinelibrary.com.]
Wang et al. Anthocyanin dyeing of cotton
fabric
© 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol.,
132, 2 2 2 –231 229
As described above, the colour
fastness to perspiration,
crocking, light, and washing of tin
mordanting dyed fabric
modified with 30 g l
1

of succinic acid was found to be

acceptable, with a grey scale
grade of at least 3.
Durability of CIELAB values and
colour strength of dyed
cotton fabrics after home
laundering
As for home laundering, the pH
value of the soapy solution
and the number of washing cycles
would greatly affect the
K/S value (Figure 9) and CIELAB
values (Table 3) of dyed
cotton fabrics. As expected, the
K/S of the fabrics decreased
with increasing number of
washing cycles. The K/S
decreased sharply even after 1
washing cycle in neutral
soapy solution (Figure 9a) and
alkaline soapy solution
(Figure 9c) for the cotton fabric
dyed without mordant tin,
and then tended to be constant,
with a K/S value of about
0.4. After five washing cycles in
alkaline soapy solution, the
K/S of cotton fabrics (Figure 9d)
with simultaneous mor-
danting dyeing also decreased to
about 0.4. However,
simultaneously mordanted and
dyed cotton fabrics (Fig-
ure 9b) retained K/S to some
extent even after 15 washing
cycles in neutral soapy solution.
Figure 9b also shows that
higher K/S values were
maintained in cotton fabrics mod-
ified with higher succinic acid
concentrations in the finish
solution. A 53.2% reduction in
K/S of cotton fabric modified
with 30 g l
1

of succinic acid in the finish

solution was still
observed after 15 laundering
cycles.
Compared with the L*, a*, and
b* values (Table 3), the
variation in the h* values was
more important in demon-
strating the colour differences of
dyed cotton fabrics after
washing, especially washing with
an alkaline soapy solu-
tion. The h* values of the control
(348.6) and modified
(343.7) cotton fabrics dyed
without mordant tin dropped to
280.8 and 273.0 as a result of
alkaline soapy solution
washing, with the colour changing
from red to light blue for
dyed cotton fabrics without
mordants. The h* values of
dyed control (313.5) and modified
(306.9) cotton fabrics
with mordant tin dropped to 288.9
and 293.6 as a result of
alkaline soapy solution washing,
with the colour changing
from deep purple (aubergine
shade) to light blue for the
control and modified cotton
fabrics. In neutral soapy
solution, on the other hand, the
colour of the dyed cotton
fabrics was more stable during
washing, especially the
colour of modified cotton fabrics
with mordant tin. The
selected dyed modified cotton
fabrics (30 g l
1

) after wash-
ing are shown in Figure 10. In
terms of colour stability of
the dyed cotton fabrics, a neutral
soapy solution was more
acceptable than an alkaline soapy
solution for washing.
The aubergine shade (deep
purple) and fastness of the
modified cotton fabrics with
mordant tin make them the
most satisfactory of the cotton
fabrics dyed with natural
anthocyanin dyes in this paper.
Conclusions
The dyeing of cotton fabric using
natural anthocyanin dyes
extracted from mulberry (Morus
rubra) was successfully
performed in this paper.
Successful modification of cotton
cellulose using succinic acid was
carried out, with little
negative effect on strength
according to the results of FTIR
analysis and tensile strength
tests. The succinic acid used to
modify cotton fabric greatly
improved the colour strength
(K/S) values and fastness of dyed
cotton fabrics. The K/S
value of dyed cotton fabric was
improved from 2.7 to 5.3 for
dyeing without mordants, and
from 3.2 to 6.9 for simulta-
neous mordanting dyeing. Red
and deep purple (aubergine)
are the two main shades of cotton
fabrics dyed with
mulberry extracts, and the
aubergine shade is rare in dyed
cotton fabrics with natural dyes.
The fastness was improved
0.5–2 grades with increasing
succinic acid concentration in
the finish solution. The colour
fastness to perspiration,
crocking, light, and washing of tin-
mordanted dyed fabric
modified with 30 g l
1

succinic acid in the finish solution

was found to be acceptable, with
a grey scale grade of at
least 3. The cotton fabrics with
simultaneous mordanting
dyeing retain their K/S values to
some extent even after 15
washing cycles in neutral soapy
solution. Moreover, the
four main anthocyanins, cyanidine
3-glucoside, cyanidine
3-rutinoside, pelargonidin 3-
glucoside, and pelargonidin 3-
rutinoside, from mulberry fruits
were separated and iden-
tified by HPLC/DAD and MS/MS
2

spectra.
References
1. T Bechtold, A Mahmudali and R
Mussak, Dyes Pigm., 75
(2007) 287.
2. S Chandravansh and S K Upadhyay,
Color. Technol., 128
(2012) 300.
3. O Deveoglu, G Erkan, E Torgan and
R Karadag, Color. Technol.,
129 (2013) 223.
4. L Wojn
arovits, C M F€
oldv
ary and E Tak
acs, Radiat. Phys.
Chem., 79 (2010) 848.
5. C S
anchez, Biotechnol. Adv., 27 (2009)
185.
6.
€
O Tunc
ß, H Tanaci and Z Aksu, J. Hazard.
Mater., 163 (2009)
187.
7. S Janhom, R Watanesk, S Watanesk,
P Griffiths, O Arquero
and W Naksata, Dyes Pigm., 71 (2006)
188.
8. A Guesmi, N Ladhari and F Sakli,
Ultrason. Sonochem., 20
(2013) 571.
9. M M Kamel, M M E Zawahry, N S E
Ahmed and F
Abdelghaffar, Ultrason. Sonochem., 16
(2009) 243.
10. M M Kamel, M M E Zawahry, N S E
Ahmed and F
Abdelghaffar, Ind. Crops Prod., 34
(2011) 1410.
11. S Rattanaphani, M Chairat, J B
Bremner and V Rattanaphani,
Dyes Pigm., 72 (2007) 88.
12. X He, R Tao, T Zhou, C Wang and
K Xie, Carbohydr. Polym.,
103 (2014) 558.
13. S Ali, T Hussain and R Nawaz, J.
Clean. Prod., 17 (2009) 61.
14. W Haddar, M B Ticha, A Guesmib,
F Khoffic and B Durand, J.
Clean. Prod., 68 (2014) 114.
15. P Velmurugan, A TamilSelvi, P
Lakshmanaperumalsamy, J
Park and B Oh, Color. Technol., 129
(2013) 246.
16. E Tsatsaroni and M Liakopoulou-
Kyriakides, Dyes Pigm., 29
(1995) 203.
17. P S Vankar, R Shanker and A
Verma, J. Clean. Prod., 15 (2007)
1441.
18. P S Vankar and R Shanker,
Desalination, 230 (2008) 62.
19. M Shahid, Shahid Ul Islam and F
Mohammad, J. Clean. Prod.,
53 (2013) 310.
20. L Liu, J Cao, J Huang, Y Cai and J
Yao, Bioresour. Technol., 101
(2010) 3268.
21. L Liu, H Lee, Y Shin, C Chyau and
C Wang, J. Food Sci., 73
(2008) H113.
22. E Pojer, F Mattivi, D Johnson and C
S Stockley, Compr. Rev.
Food Sci. Food Saf., 12 (2013) 483.
23. E J Kwak, J Y Lee and I S Choi, J.
Food Sci., 77 (2012) C752.
24. J Chen, J Kan, J Tang, Z Cai and J
Liu, J. Food Sci., 77 (2012)
C430.
25. G Hojjatpanah, M Fazaeli and Z
Emam-Djomeh, Int. J. Food
Sci. Tech., 46 (2011) 956.
26. J M Awika, L W Rooney and R D
Waniska, Food Chem., 90
(2005) 293.
27. M P Doyle, F F Busta, B Cord and P
Davidson, Compr. Rev.
Food Sci. Food Saf., 5 (2006) 71.
28. G Agati and M Tattini, New
Phytol., 186 (2010) 786.
Wang et al. Anthocyanin dyeing of cotton
fabric
230 © 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol., 132,
222–231
29. W J Steyn, S J E Wand, G Jacobs, R
C Rosecrance and S C
Roberts, Physiol. Plant., 136 (2009)
461.
30. F C Stintzing and R Carle, Trends
FoodSci. Technol., 15 (2004) 19.
31. U Szymanowska, U Zlotek, M
Karas and B Baraniak, Food
Chem., 172 (2015) 71.
32. E Sadilova, R Carle and F C
Stintzing, Mol. Nutr. Food Res., 51
(2007) 1461.
33.
€
O Turfan, M T€
urkyilmaz, O Yemis and M
€
Ozkanb, Food
Chem., 129 (2011) 1644.
34. I S Kang, C Q Yang, W Wei and G C
Lickfield, Text. Res. J., 68
(1998) 865.
35. ASTM D5035-11(2015) Standard
test method for breaking force
and elongation of textile fabrics (strip
method) (West Con-
shohoken, PA: ASTM International,
2015).
36. AATCC 16-2004 Colorfastness to
light (Research Triangle Park,
NC: AATCC, 2004).
37. AATCC 61-2009 Colorfastness to
laundering: accelerated
(Research Triangle Park, NC: AATCC,
2009).
38. AATCC 8-2007 Colorfastness to
crocking (Research Triangle
Park, NC: AATCC, 2007).
39. AATCC 15-2009 Colorfastness to
perspiration (Research Trian-
gle Park, NC: AATCC, 2009).
40. AATCC 61(2A)-2009 Colorfastness
to laundering, home and
commercial: accelerated (machine
wash) (Research Triangle
Park, NC: AATCC, 2009).
41. R Badulescu, V Vivod, D Jausovec
and B Voncina, Carbohydr.
Polym., 71 (2008) 85.
42. C Q Yang, W Zhou, G C Lickfield
and K Parachura, Text. Res. J.,
73 (2013) 1057.
43. M P Gashti, A Elahi and M P Gashti,
Compos. Eng., B48 (2013)
158.
44. G Crini and P M Badot, Prog.
Polym. Sci., 33 (2008) 399.
45. G A Ellestad, Chirality, 18 (2006)
134.
46. J A Hernandez-Herrero and M J
Frutos, Food Chem., 154 (2014)
199.
47. T K McGhie and M C Walton, Mol.
Nutr. Food Res., 51 (2007)
702.
48. C Q Yang, Text. Res. J., 71 (2001)
201.
49. S R Maulik, D Das and S C
Bhattacharya, J. Text. Inst., 102
(2011) 131.
50. J Parrado, M L Escudero-Gilete, V
Friaza, A Garc
ıa-Mart
ınez,
M L Gonz
alez-Miret, J D Bautista and F J
Heredia, J. Sci. Food
Agric., 87 (2007) 2310.
51. Y S Oh, J H Lee, S H Yoon, C H Oh,
D S Choi, E Choe and M Y
Jung, J. Food Sci., 73 (2008) C378.
52. T Zou, D Wang, H Guo, Y Zhu, X
Luo, F Liu and W Ling, J.
Food Sci., 77 (2012) C46.
53. Y Chen, W Zhang, T Zhao, F Li, M
Zhang, J Li, Y Zou, W
Wang, S J Cobbina, X Wu and L Yang,
Food Chem., 194 (2016)
712.
54. A Casta~
neda-Ovando, M L Pacheco-Hern
andez, M E P
aez-
Hern
andez, J A Rodr
ıguez and C A Gal
an-Vidal, Food Chem.,
113 (2009) 859.
55. T Goto, H Tamura, T Kawai, T
Hoshino, N Harada and T
Kondo, Ann. NY Acad. Sci., 471 (1986)
155.
56. R N Cavalcanti, D T Santos and M
A A Meireles, Food Res. Int.,
44 (2011) 499.
57. K Han, T Kitano-Okada, J Seo, S
Kim, K Sasaki, K Shimada and
M Fukushima, J. Funct. Foods, 14
(2015) 692.
58.
€
O E Ismal, Color. Technol., 130 (2014)
147.
59.
€
O E Ismal, E
€
Ozdogan and L Yildirim, Color.
Technol., 129
 (2013) 431.
Wang et al. Anthocyanin dyeing of cotton
fabric
© 2016 The Authors. Coloration
Technology © 2016 Society of Dyers
and Colourists, Colora. Technol.,
132, 2 2 2 –231 231
Citations (8)
References (90)
 Non-conventional Plant Fibres
Chapter

o Jan 2019
o

Majda Sfiligoj Smole

Silvo Hribernik

Manja Kurecic

Karin Stana-Kleinschek

View
Show abstract
 Dyeing of cotton with the natural dye extracted from waste leaves of
green tea ( Camellia sinensis var. assamica )

Article

o Dec 2018
o COLOR TECHNOL
o

Sukemi Sukemi

o Kornkanya Pratumyot
o Choladda Srisuwannaket
o

Withawat Mingvanish

View
Show abstract

 Complexation of common metal cations by cyanins: Binding affinity and

molecular structure

Article

o Nov 2018
o INT J QUANTUM CHEM
o
 Laura Estévez

o Marta Sánchez-Lozano
o

Ricardo Mosquera

View
Show abstract

 A physicochemical characterisation of a medieval herbal ink, Mahī, of

Assam, India

Article

o Jul 2018
o COLOR TECHNOL
o

Barsha RITU Goswami

Nabadweep Chamuah

o
 Robin Dutta

View
Show abstract

 Review on Methods and Technologies for Improvement of Adsorption and

Fastness Properties of Natural Dyes on Cotton Fibers

Article
Full-text available

o Jan 2017
o

Aminoddin Haji

View
Show abstract

 Antibacterial cotton fabric with enhanced durability prepared using L-

cysteine and silver nanoparticles

Article

o Nov 2017
o FIBER POLYM
o QingBo Xu
o Jiayuan Gu
o Yang Zhao
o
 Xiangdong Liu

View
Show abstract

 Natural Colorants: Historical, Processing and Sustainable Prospects

Article
Full-text available

o Jan 2017
o

Mohd Yusuf

Mohd Shabbir

Faqeer Mohammad

View
Show abstract
 Effect of water pressure on mechanical behavior of concrete under
dynamic compression state

Article

o Oct 2016
o CONSTR BUILD MATER
o Qianfeng Wang
o Yunhe Liu
o Gang Peng

View

Show abstract

 Show more